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Carbon Based Electrochemical Sensors with Nafion Coating for Selective Detection of Drug Molecules E

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Carbon Based Electrochemical Sensors with Nafion Coating for Selective Detection of Drug Molecules E [P13.01] Carbon based electrochemical sensors with nafion coating for selective detection of drug molecules E. Mynttinen* 1, N. Wester 1, J. Etula 1, E. Kauppinen 1, E. Kalso 2,3 , T. Lilius 2, J. Koskinen 1, T. Laurila 1 1Aalto University, Finland, 2University of Helsinki, Finland, 3Helsinki University Hospital, Finland Novel carbon materials, such as tetrahedral amorphous carbon (ta-C) and various carbon nanostructures, have shown great promise in sensitive and selective electrochemical detection of biological molecules [1,2]. The selectivity of such sensors can be further improved with cation exchange polymers, such as Nafion, exhibiting permselective properties [3]. In hospital environments, accurate determination of drug molecule concentrations is essential in pain management for efficient and safe dosing. However, the current analysis methods are both time consuming and laborious, and are thus not sufficient for adaptive pain treatment. For this purpose, carbon based electrochemical sensors coated with permselective Nafion films can enable fast and effortless detection without compromising sensitivity and selectivity. The permselective properties of Nafion appear to be affected by differences in the surface roughness of the electrode, and thus the selectivity of the sensor could be tailored by modifying its topography. We have generated two types of carbon based thin film electrodes coated with Nafion for the detection of biological molecules: a smooth ta-C surface and a carbon nanotube (CNT) thin film with larger surface roughness. In this work, we will evaluate the effect of surface roughness of the underlying carbon material on the permselective properties with cyclic voltammetry (CV) and differential pulse voltammetry (DPV). The physical, chemical and electrochemical properties of ta-C electrodes have been characterized in detail in previous work [1,4,5]. The electrochemical properties of the prepared Nafion coated sensors will be assessed with several outer and inner sphere probes. In addition, the materials will be characterized by SEM, AFM and Raman spectroscopy. The sensor performance will be evaluated with various biological molecules (Fig.1). It is anticipated that with these novel electrode materials, fast, sensitive and selective detection of various drug molecules with clinical relevance can be achieved. Figure 1. Differential pulse voltammograms for ta-C and ta-C coated with Nafion in 500 µM of AA and UA (A) and 50 µM PA (B). ta-C coated with Nafion (C) and CNT coated with Nafion (D) in 500 µM of AA and UA and 10 µM MO. On ta-C, the polymer film greatly reduces the signals of AA and UA (A) while still preserving its ability to detect PA (B). However, this sensor completely fails to detect MO (C), in contrast to the nanostructured surface (D). On the other hand, the CNT sensor seems to have an unfavorable response for UA and PA in respect to each other, compared to that of ta-C. 1. Laurila, T., et al. "New electrochemically improved tetrahedral amorphous carbon films for biological applications". Diamond and Related Materials 49 (2014): 62-71. 2. Sainio, S., et al. “Integrated Carbon Nanostructures for Detection of Neurotransmitters”. Molecular Neurobiology 52 (2015): 859-866. 3. Ribeiro, J. A., “Electrochemical sensors and biosensors for determination of catecholamine neurotransmitters: A review”. Talanta 160 (2016): 653-679. 4. Protopopova, V. S., et al. "Ultrathin undoped tetrahedral amorphous carbon films: thickness dependence of the electronic structure and implications for their electrochemical behaviour". Physical Chemistry Chemical Physics 17.14 (2015): 9020-9031. 5. Palomäki, T., et al. "Electron transport determines the electrochemical properties of tetrahedral amorphous carbon (ta-C) thin films". Electrochimica Acta 225 (2017): 1-10. Keywords: Carbon nanotube, Tetrahedral amorphous carbon, Electrochemical sensor, Nafion [P13.02] Carbon coated GaN sensors I.B. Usman*, N.J. Coville, B.W. Mwakikunga, D.M. Wamwangi University of the Witwatersrand, South Africa Gallium nitride (GaN) is a wide-band gap (3.39 eV) semiconductor with excellent thermal stability for applications in optoelectronic devices [1 - 3]. As sensors GaN does not operate at room temperature. In this study carbon coated GaN nanostructures are investigated for the role of carbon defects in room temperature sensor applications. The optical and electronic properties of defects in GaN is of great importance for evaluating the degree to which they affect the devices’ performance. The carbon coated GaN (C-GaN) was synthesised using a horizontal chemical vapour deposition (CVD) setup at 600 °C. The physico-chemical properties of the C- GaN have been carried using XRD, TEM, SEM, TGA, Raman, PL and XPS procedures to establish the disorder of the carbon on the surface of GaN. TGA showed that more carbon is coated on the surface of GaN when argon was used as a carrier gas compared to nitrogen. The PL spectrum of C-GaN showed that the intensity of the YL peaks for all the samples containing carbon is suppressed compared to pure GaN. This is attributed to anti site (C N) defects. As a proof of concept C-GaN were tested for gas sensing applications through measurements of the change in electrical resistance of the C-GaN as a function of analyte composition (0-100 ppm) at varying temperatures (300K-500K). The results will be described. REFERENCES 1. X.M. Cai, et al., Thin Solid Films, 2006. 515 2. F. Choa et al., Appl. Phys. Lett., 1996. 69(24); S. Nakamura et al., Jpn. J. Appl. Phys., 1997. 36 3. R. Armitage et al., Appl. Phys. Lett. 92 (2002) 2575 Keywords: Carbon coated GaN, TGA, PL [P13.03] Development of the direct methanol fuel cell electrocatalyst using marimo nano carbon as a novel electrode material K. Saito* 1, K. Nakagawa 1,2 , T. Ando 3 1Kansai University, Japan, 2HRC, Japan, 3NIMS, Japan Direct methanol fuel cell (DMFC) uses a carbon supported Pt catalyst for electrode. Carbon black is generally used the catalyst support material. However, a lot of Pt particle was loaded in the inner micro pore of carbon black. Because methanol cannot get into the micro pore, the activity of Pt loading carbon black catalyst is not high. Therefore, we demonstrated marimo nano carbon (MNC) for a novel catalyst support material. MNC is spherical carbon nanofilaments (CNFs). CNFs were synthesized radially from oxidized diamond (O-dia) supported catalysts for the core. MNC has meso size interfiber voids. We expected Pt particle supported inside of MNC was effective, evaluated the catalyst activity and power generation performance. MNCs were synthesized by CCVD method. Ni/O-dia and Co/O-dia were used as catalysts. Pt supported on MNCs was prepared by the modified nanocolloidal method. Pt supported on Vulcan XC72 (carbon black: CABOT) was also prepared for comparison. Pt loading level was 5 wt%. The catalyst activity was measured by cyclic voltammetly measurements (CV). The I-V performances were measured by unit cell for DMFC. The Pt metal state was analysed using X- ray photoelectron spectroscopy (XPS). Figure 1 shows cyclic voltammograms of Pt loading catalysts. Methanol oxidation reaction peaks were observed in the region of 0.6 V. The peak current density of Pt/MNC(Ni) was the highest. Figure 2 shows the results of I-V measurement. The max power density of unit cell using Pt/MNC(Ni) in both electrode was the highest. Figure 3 shows the XPS spectra of Pt4f in the Pt loading catalysts. Pt peak intensity was the highest when using MNC(Ni) for catalyst support. Because electrochemically active Pt was supported on the surface of CNFs. ] 200 0.4 Pt/MNC(Ni) Pt Pt/MNC(Ni) Pt/MNC(Ni) Pt/MNC(Co) Pt/MNC(Co) Pt/MNC(Co) 4f 7/2 Pt/Vulcan 0.3 Pt/Vulcan Pt/Vulcan 4f 5/2 100 0.2 Intensity [-] Voltage [V] Voltage 0.1 0 Current density [mA/mg density Current 0 -0.2 0 0.2 0.4 0.6 0.8 1 1.2 0 2 4 6 8 78 76 74 72 70 Voltage [V] Current density [mA/cm 2] Binding Energy [eV] Fig.1 Cyclic voltammograms of Pt loading catalysts. Fig.2 I-V characteristic of DMFC. Fig.3 XPS spectra of Pt4f on Pt loading catalysts. Using MNC(Ni) as catalyst support, the Pt catalyst activity and the power generation performance of DMFC was increased. Keywords: Marimo nano carbon, Direct methanol fuel cell, Oxidized diamond, Carbon nanofilament [P13.04] Oxygen Reduction Reaction on N-doped activated carbons obtained from chitin and chitosan A. Ilnicka* 1, J.P. Lukaszewicz 1, K. Shimanoe 2, M. Yuasa 3 1Nicolaus Copernicus University, Poland, 2Kyushu University, Japan, 3Kindai University, Japan Recently, porous carbon materials doped with heteroatoms, such as oxygen and nitrogen have attracted considerable attention to some electrochemical energy devices (supercapacitors, fuel cells, metal-air batteries) due to several unique properties of heteroatom incorporating surface active sites. In this research we used chitin and chitosan as the carbon source to synthesize the N-doping catalysts. Chitin and chitosan were subjected to an different activation procedures. In order to improve the electrocatalytic activity, the prepared catalyst is further subjected to the urea impregnation. Then, the nitrogen sorption isotherm, scanning electron microscopy, elemental analysis, and X- ray photoelectron spectroscopy were used to study the microstructure and composition. The catalytic voltammetry and rotating-ring-disk electrode methods were used to investigate the electrochemical behaviour for the oxygen reduction reaction (ORR). The research presents how urea-treatment influenced several textural, chemical and electrocatalytic properties of N-doped activated carbons obtained from renewal resources like chitosan and chitin. The urea-treatment resulted in a spectacular increase in nitrogen content by weight (up to 68%) and the improvement of the surface area (up to 42%) along with total/micro-/mezo- pore volume (up to 49%). In summary, we have, for the first time, prepared N-doping carbon materials with or without urea from chitin and chitosan.
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